A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Abstract The rational design and control of electrocatalysts at single‐atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi‐Rh 1 ) by atomic galvanic replacement, and their subsequent transformation into a tensile‐strained Pt–Rh single‐atom alloy (PtBi@PtRh 1 ) via electrochemical dealloying are presented. Benefiting from the Rh 1 ‐tailored Pt (110) surface with tensile strain, the PtBi@PtRh 1 nanoplates exhibit record‐high and all‐round superior electrocatalytic performance including activity, selectivity, stability, and anti‐poisoning ability toward ethanol oxidation in alkaline electrolytes. Density functional theory calculations reveal the synergism between effective Rh 1 and tensile strain in boosting the adsorption of ethanol and key surface intermediates and the CC bond cleavage of the intermediates. The facile synthesis of the tensile‐strained single‐atom alloy provides a novel strategy to construct model nanostructures, accelerating the development of highly efficient electrocatalysts.